Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis

Matteo Monai, Kellie Jenkinson, Angela E M Melcherts, Jaap N Louwen, Ece A Irmak, Sandra Van Aert, Thomas Altantzis, Charlotte Vogt, Ward van der Stam, Tomáš Duchoň, Břetislav Šmíd, Esther Groeneveld, Peter Berben, Sara Bals, Bert M Weckhuysen

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiO x overlayers formed on nickel/titanium dioxide catalysts during 400°C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600°C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiO x and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships.

Original languageEnglish
Pages (from-to)644-651
Number of pages8
JournalScience (New York, N.Y.)
Volume380
Issue number6645
DOIs
Publication statusPublished - 12 May 2023

Bibliographical note

Publisher Copyright:
Copyright © 2023 the authors, some rights reserved.

Funding

This work was supported by BASF and NWO CHIPP (research grant to B.M.W.); the MCEC NWO Gravitation Program (B.M.W.); the ARC-CBBC NWO Program (B.M.W.); the European Research Council (grant 770887 PICOMETRICS to S.V.A.); and the European Research Council (grant 815128 REALNANO to S.B.).

FundersFunder number
ARC-CBBC NWO
MCEC NWO
BASF
European Research Council815128, 770887 PICOMETRICS
Nederlandse Organisatie voor Wetenschappelijk Onderzoek

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